Journal of Chemical Physics, volume 150, issue 12, pages 124502
Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal
1
Department of Chemical and Biomolecular Engineering, University of Pennsylvania 1 , Philadelphia, Pennsylvania 19104, USA
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Publication type: Journal Article
Publication date: 2019-03-22
Journal:
Journal of Chemical Physics
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 4.4
ISSN: 00219606, 10897690
Physical and Theoretical Chemistry
General Physics and Astronomy
Abstract
In this work, we use large-scale molecular dynamics simulations coupled to free energy calculations to identify for the first time a limit of stability (spinodal) and a change in the nucleation mechanism in aqueous NaCl solutions. This is a system of considerable atmospheric, geological, and technical significance. We find that the supersaturated metastable NaCl solution reaches its limit of stability at sufficiently high salt concentrations, as indicated by the composition dependence of the salt chemical potential, indicating the transition to a phase separation by spinodal decomposition. However, the metastability limit of the NaCl solution does not correspond to spinodal decomposition with respect to crystallization. We find that beyond this spinodal, a liquid/amorphous separation occurs in the aqueous solution, whereby the ions first form disordered clusters. We term these clusters as “amorphous salt.” We also identify a transition from one- to two-step crystallization mechanism driven by a spinodal. In particular, crystallization from aqueous NaCl solution beyond the spinodal is a two-step process, in which the ions first phase-separate into disordered amorphous salt clusters, followed by the crystallization of ions in the amorphous salt phase. By contrast, in the aqueous NaCl solution at concentrations lower than the spinodal, crystallization occurs via a one-step process as the ions aggregate directly into crystalline nuclei. The change of mechanism with increasing supersaturation underscores the importance of an accurate determination of the driving force for phase separation. The study has broader implications on the mechanism for nucleation of crystals from solutions at high supersaturations.
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Wiley
1 publication, 1.45%
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Springer Nature
1 publication, 1.45%
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- We do not take into account publications that without a DOI.
- Statistics recalculated only for publications connected to researchers, organizations and labs registered on the platform.
- Statistics recalculated weekly.
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Jiang H., Debenedetti P., Panagiotopoulos A. Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal // Journal of Chemical Physics. 2019. Vol. 150. No. 12. p. 124502.
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Jiang H., Debenedetti P., Panagiotopoulos A. Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal // Journal of Chemical Physics. 2019. Vol. 150. No. 12. p. 124502.
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TY - JOUR
DO - 10.1063/1.5084248
UR - https://doi.org/10.1063/1.5084248
TI - Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal
T2 - Journal of Chemical Physics
AU - Jiang, Hao
AU - Debenedetti, P.G
AU - Panagiotopoulos, A.Z.
PY - 2019
DA - 2019/03/22 00:00:00
PB - American Institute of Physics (AIP)
SP - 124502
IS - 12
VL - 150
SN - 0021-9606
SN - 1089-7690
ER -
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@article{2019_Jiang,
author = {Hao Jiang and P.G Debenedetti and A.Z. Panagiotopoulos},
title = {Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal},
journal = {Journal of Chemical Physics},
year = {2019},
volume = {150},
publisher = {American Institute of Physics (AIP)},
month = {mar},
url = {https://doi.org/10.1063/1.5084248},
number = {12},
pages = {124502},
doi = {10.1063/1.5084248}
}
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Jiang, Hao, et al. “Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal.” Journal of Chemical Physics, vol. 150, no. 12, Mar. 2019, p. 124502. https://doi.org/10.1063/1.5084248.